Argon offline-AMS source apportionment of organic aerosol over yearly cycles for an urban, rural, and marine site in northern Europe

Bozzetti, Carlo; Sosedova, Yulia; Xiao, Mao; Daellenbach, Kaspar R.; Ulevičius, Vidmantas; Dudoitis, Vadimas; Mordas, Genrik; Byčenkienė, Steigvilė; Plauškaitė, Kristina; Vlachou, Athanasia; Golly, B.; Chazeau, Benjamin; Besombes, Jean-Luc; Baltensperger, Urs; Jaffrezo, Jean-Luc; Slowik, Jay G.; Haddad, Imad El; Prévôt, And André S. H.

doi:10.5194/acp-17-117-2017

Cited by 71 publications

(59 citation statements)

References 76 publications

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“…4e and f), and the relation to markers (Fig. 5c and d) of the two factors are in agreement with those from earlier work at other locations, including Zürich (Daellenbach et al, 2016), Payerne , and Lithuania (Bozzetti et al, 2017a). This OOA separation appears to be typical for PMF analysis of long-term, low-timeresolution OA mass spectra of filter samples.…”

Section: Interpretation Of Pmf Factorssupporting

confidence: 78%

“…The measurement blank was subtracted from the sample spectra. In a previous study, it has been shown that the measurement blank is comparable to the organic blanks obtained from the nebulization of NH 4 NO 3 (Bozzetti et al, 2017a …”

Section: Offline Ams Analysismentioning

confidence: 99%

“…This approach allows the retroactive investigation of specific events, e.g. haze events in China , as well as AMS measurements of coarse-mode aerosol and long-term source apportionment studies (Bozzetti, 2017a, b). Such an approach was also used in recent studies for identifying the different types of water-soluble chromophores (Chen et al, 2016).…”

Section: Introductionmentioning

confidence: 99%

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Long-term chemical analysis and organic aerosol source apportionment at nine sites in central Europe: source identification and uncertainty assessment

et al. 2017

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Abstract. Long-term monitoring of organic aerosol is important for epidemiological studies, validation of atmospheric models, and air quality management. In this study, we apply a recently developed filter-based offline methodology using an aerosol mass spectrometer (AMS) to investigate the regional and seasonal differences of contributing organic aerosol sources. We present offline AMS measurements for particulate matter smaller than 10 µm at nine stations in central Europe with different exposure characteristics for the entire year of 2013 (819 samples). The focus of this study is a detailed source apportionment analysis (using positive matrix factorization, PMF) including in-depth assessment of the related uncertainties. Primary organic aerosol (POA) is separated in three components: hydrocarbon-like OA related to traffic emissions (HOA), cooking OA (COA), and biomass burning OA (BBOA). We observe enhanced production of secondary organic aerosol (SOA) in summer, following the increase in biogenic emissions with temperature (summer oxygenated OA, SOOA). In addition, a SOA component was extracted that correlated with an anthropogenic secondary inorganic species that is dominant in winter (winter oxygenated OA, WOOA). A factor (sulfur-containing organic, SC-OA) explaining sulfur-containing fragments (CH 3 SO + 2 ), which has an event-driven temporal behaviour, was also identified. The relative yearly average factor contributions range from 4 to 14 % for HOA, from 3 to 11 % for COA, from 11 to 59 % for BBOA, from 5 to 23 % for SC-OA, from 14 to 27 % for WOOA, and from 15 to 38 % for SOOA. The uncertainty of the relative average factor contribution lies between 2 and 12 % of OA. At the sites north of the alpine crest, the sum of HOA, COA, and BBOA (POA) contributes less to OA (POA / OA = 0.3) than at the southern alpine valley sites (0.6). BBOA is the main contributor to POA with 87 % in alpine valleys and 42 % north of the alpine crest. Furthermore, the influence of primary biological particles (PBOAs), not resolved by PMF, is estimated and could contribute significantly to OA in PM 10 .

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Section: Interpretation Of Pmf Factorssupporting

confidence: 78%

Section: Offline Ams Analysismentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Long-term chemical analysis and organic aerosol source apportionment at nine sites in central Europe: source identification and uncertainty assessment

et al. 2017

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“…We note that while the assessment of the uncertainties related to the O : C measurements by the HR-ToF-AMS is not straightforward, a distinction should be made between measurement precision and accuracy. We do not expect the accuracy of the O : C ratios determined by the HR-ToF-AMS to be less than ∼ 20 % (Aiken et al, 2008;Pieber et al, 2016;Canagaratna et al, 2015;Bozzetti et al, 2017). For example, the use of a more recent parameterization would yield higher O : C values (by 18 %) and the O : C ratios reported here may be regarded as the lowest estimates.…”

Section: Experimental Set-up and Instrumentationmentioning

confidence: 67%

Assessing the influence of NOx concentrations and relative humidity on secondary organic aerosol yields from α-pinene photo-oxidation through smog chamber experiments and modelling calculations

et al. 2017

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Abstract. Secondary organic aerosol (SOA) yields from the photo-oxidation of α-pinene were investigated in smog chamber (SC) experiments at low (23-29 %) and high (60-69 %) relative humidity (RH), various NO x / VOC ratios (0.04-3.8) and with different aerosol seed chemical compositions (acidic to neutralized sulfate-containing or hydrophobic organic). A combination of a scanning mobility particle sizer and an Aerodyne high-resolution time-of-flight aerosol mass spectrometer was used to determine SOA mass concentration and chemical composition. We used a Monte Carlo approach to parameterize smog chamber SOA yields as a function of the condensed phase absorptive mass, which includes the sum of OA and the corresponding bound liquid water content. High RH increased SOA yields by up to 6 times (1.5-6.4) compared to low RH. The yields at low NO x / VOC ratios were in general higher compared to yields at high NO x / VOC ratios. This NO x dependence follows the same trend as seen in previous studies for α-pinene SOA.A novel approach of data evaluation using volatility distributions derived from experimental data served as the basis for thermodynamic phase partitioning calculations of model mixtures in this study. These calculations predict liquidliquid phase separation into organic-rich and electrolyte phases. At low NO x conditions, equilibrium partitioning between the gas and liquid phases can explain most of the increase in SOA yields observed at high RH, when in addition to the α-pinene photo-oxidation products described in the literature, fragmentation products are added to the model mixtures. This increase is driven by both the increase in the absorptive mass and the solution non-ideality described by the compounds' activity coefficients. In contrast, at high NO x , equilibrium partitioning alone could not explain the strong increase in the yields with RH. This suggests that other processes, e.g. reactive uptake of semi-volatile species into the liquid phase, may occur and be enhanced at higher RH, especially for compounds formed under high NO x conditions, e.g. carbonyls.

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“…The recent utilization of the AMS for the offline analysis of ambient filter samples has significantly broadened the spatial and temporal scales accessible to high-resolution AMS measurements (Daellenbach et al, 2017;Bozzetti et al, 2017a, b). In addition, the technique enables measurement of aerosol composition outside the normal size transmission window of the AMS; the standard AMS can measure up to only 1 µm, or ∼ 2.5 µm with a newly developed aerodynamic lens (Williams et al, 2013;Elser et al, 2016).…”

Section: Introductionmentioning

confidence: 99%

Advanced source apportionment of carbonaceous aerosols by coupling offline AMS and radiocarbon size-segregated measurements over a nearly 2-year period

et al. 2018

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Abstract. Carbonaceous aerosols are related to adverse human health effects. Therefore, identification of their sources and analysis of their chemical composition is important. The offline AMS (aerosol mass spectrometer) technique offers quantitative separation of organic aerosol (OA) factors which can be related to major OA sources, either primary or secondary. While primary OA can be more clearly separated into sources, secondary (SOA) source apportionment is more challenging because different sources -anthropogenic or natural, fossil or non-fossil -can yield similar highly oxygenated mass spectra. Radiocarbon measurements provide unequivocal separation between fossil and non-fossil sources of carbon. Here we coupled these two offline methods and analysed the OA and organic carbon (OC) of different size fractions (particulate matter below 10 and 2.5 µm -PM 10 and PM 2.5 , respectively) from the Alpine valley of Magadino (Switzerland) during the years 2013 and 2014 (219 samples). The combination of the techniques gave further insight into the characteristics of secondary OC (SOC) which was rather based on the type of SOC precursor and not on the volatility or the oxidation state of OC, as typically considered. Out of the primary sources separated in this study, biomass burning OC was the dominant one in winter, with average concentrations of 5.36 ± 2.64 µg m −3 for PM 10 and 3.83 ± 1.81 µg m −3 for PM 2.5 , indicating that wood combustion particles were predominantly generated in the fine mode. The additional information from the size-segregated measurements revealed a primary sulfur-containing factor, mainly fossil, detected in the coarse size fraction and related to non-exhaust traffic emissions with a yearly average PM 10 (PM 2.5 ) concentration of 0.20 ± 0.24 µg m −3 (0.05 ± 0.04 µg m −3 ). A primary biological OC (PBOC) was also detected in the coarse mode peaking in spring and summer with a yearly average PM 10 (PM 2.5 ) concentration of 0.79 ± 0.31 µg m −3 (0.24 ± 0.20 µg m −3 ). The secondary OC was separated into two oxygenated, non-fossil OC factors which were identified based on their seasonal variability (i.e. summer and winter oxygenated organic carbon, OOC) and a third anthropogenic OOC factor which correlated with fossil OC mainly peaking in winter and spring, contributing on average 13 % ± 7 % (10 % ± 9 %) to the total OC in PM 10 (PM 2.5 ). The winter OOC was also connected to anthropogenic sources, contributing on average 13 % ± 13 % (6 % ± 6 %) to the total OC in PM 10 (PM 2.5 ). The summer OOC (SOOC), stemming from oxidation of biogenic emissions, was more pronounced in the fine mode, contributing on average 43 % ± 12 % (75 % ± 44 %) to the total OC in PM 10 (PM 2.5 ). In total the non-fossil OC significantly dominated the fossil OC throughout all seasons, by contributing on average 75 % ± 24 % to the total OC. The results also suggested that during the cold period the prevailing source was residential biomass burning while during the warm period primaryPublished by Copernicus Publications o...

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Argon offline-AMS source apportionment of organic aerosol over yearly cycles for an urban, rural, and marine site in northern Europe

Abstract: International audienc

Cited by 71 publications

References 76 publications

Long-term chemical analysis and organic aerosol source apportionment at nine sites in central Europe: source identification and uncertainty assessment

Long-term chemical analysis and organic aerosol source apportionment at nine sites in central Europe: source identification and uncertainty assessment

Assessing the influence of NO<sub><i>x</i></sub> concentrations and relative humidity on secondary organic aerosol yields from <i>α</i>-pinene photo-oxidation through smog chamber experiments and modelling calculations

Advanced source apportionment of carbonaceous aerosols by coupling offline AMS and radiocarbon size-segregated measurements over a nearly 2-year period

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Argon offline-AMS source apportionment of organic aerosol over yearly cycles for an urban, rural, and marine site in northern Europe

Abstract: International audienc

Cited by 71 publications

References 76 publications

Long-term chemical analysis and organic aerosol source apportionment at nine sites in central Europe: source identification and uncertainty assessment

Long-term chemical analysis and organic aerosol source apportionment at nine sites in central Europe: source identification and uncertainty assessment

Assessing the influence of NO&lt;sub&gt;&lt;i&gt;x&lt;/i&gt;&lt;/sub&gt; concentrations and relative humidity on secondary organic aerosol yields from &lt;i&gt;α&lt;/i&gt;-pinene photo-oxidation through smog chamber experiments and modelling calculations

Advanced source apportionment of carbonaceous aerosols by coupling offline AMS and radiocarbon size-segregated measurements over a nearly 2-year period

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Assessing the influence of NO<sub><i>x</i></sub> concentrations and relative humidity on secondary organic aerosol yields from <i>α</i>-pinene photo-oxidation through smog chamber experiments and modelling calculations